文献类型：期刊文献

英文题名：Identifying the distinct features of geometric structures for hole trapping to generate radicals on rutile TiO2(110) in photooxidation using density functional theory calculations with hybrid functional

作者：Wang, Dong[1,2,3];Wang, Haifeng[1,2];Hu, P.[1,2,3]

机构：[1]E China Univ Sci & Technol, Ctr Computat Chem, Key Lab Adv Mat, Shanghai 200237, Peoples R China;[2]E China Univ Sci & Technol, Res Inst Ind Catalysis, Shanghai 200237, Peoples R China;[3]Queens Univ Belfast, Sch Chem & Chem Engn, Belfast BT9 5AG, Antrim, North Ireland

年份：2015

卷号：17

期号：3

起止页码：1549

外文期刊名：PHYSICAL CHEMISTRY CHEMICAL PHYSICS

收录：;WOS:【SCI-EXPANDED(收录号:WOS:000346473600002)】；

基金：This project is supported by National Natural Science Foundation of China (21303052, 21333003), Fundamental Research Funds for the Central Universities (222201314035), the Commission of Science and Technology of Shanghai Municipality (12ZR1442600), Shanghai Rising-Star Program (14QA1401100), Fund for Innovative Research Groups of Natural Science Foundation of China (21321004). D. W. thanks the Chinese Scholarship Council for the abroad living support and P. H. thanks the Chinese Government for the "Thousands Talents'' program.

语种：英文

摘要：Using density functional theory calculations with HSE 06 functional, we obtained the structures of spin-polarized radicals on rutile TiO2(110), which is crucial to understand the photooxidation at the atomic level, and further calculate the thermodynamic stabilities of these radicals. By analyzing the results, we identify the structural features for hole trapping in the system, and reveal the mutual effects among the geometric structures, the energy levels of trapped hole states and their hole trapping capacities. Furthermore, the results from HSE 06 functional are compared to those from DFT + U and the stability trend of radicals against the number of slabs is tested. The effect of trapped holes on two important steps of the oxygen evolution reaction, i.e. water dissociation and the oxygen removal, is investigated and discussed.